CN101847522B - Electric double layer capacitor - Google Patents

Electric double layer capacitor Download PDF

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Publication number
CN101847522B
CN101847522B CN201010142554.7A CN201010142554A CN101847522B CN 101847522 B CN101847522 B CN 101847522B CN 201010142554 A CN201010142554 A CN 201010142554A CN 101847522 B CN101847522 B CN 101847522B
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double layer
capacitor
anionic polymer
polyacid
particulate
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CN101847522A (en
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德克·H·德赖西格
乔纳森·R·克诺普斯尼德
杰西卡·M·史密斯
李·希纳伯格
巴拉特·拉瓦尔
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Kyocera AVX Components Co.,Ltd.
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AVX Corp
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/22—Electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/04—Hybrid capacitors
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/22—Electrodes
    • H01G11/24—Electrodes characterised by structural features of the materials making up or comprised in the electrodes, e.g. form, surface area or porosity; characterised by the structural features of powders or particles used therefor
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/54—Electrolytes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/54—Electrolytes
    • H01G11/58—Liquid electrolytes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/54—Electrolytes
    • H01G11/58—Liquid electrolytes
    • H01G11/62—Liquid electrolytes characterised by the solute, e.g. salts, anions or cations therein
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/54—Electrolytes
    • H01G11/58—Liquid electrolytes
    • H01G11/64—Liquid electrolytes characterised by additives
    • H01G9/038—
    • H01G9/155—
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/13—Energy storage using capacitors

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  • Engineering & Computer Science (AREA)
  • Power Engineering (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Materials Engineering (AREA)
  • Electric Double-Layer Capacitors Or The Like (AREA)

Abstract

An electric double layer capacitor that contains at least one electrochemical cell is provided. The cell contains electrodes (e.g., two electrodes) that each contain a porous matrix of electrochemically-active particles (e.g., carbon). An aqueous-based electrolyte is disposed in contact with the porous matrix. In accordance with the present invention, the electrolyte is provided with an anionic polymer that serves as binding agent for the electrochemically active particles and thus reduces electrolyte loss, especially at higher temperatures. Because the polymer is anionic in nature, it is generally hydrophilic and thus can retain its binding properties in the presence of water. The anionic nature of the polymer also allows it to remain stable in the presence of a corrosive polyprotic acid, which is employed in the electrolyte to enhance charge density. Thus, as a result of the present invention, a capacitor may be formed that is capable of exhibiting good electrical performance (e.g., high capacitance and low ESR), even at high temperatures (e.g., 70 DEG C. and above).

Description

Double layer capacitor
Background technology
Double layer capacitor uses a pair polarizable electrode usually, and this polarizable electrode comprises a porous matrix formed by electrically conductive particles (such as, activated carbon).Porous matrix is injected into liquid electrolyte, and this electrolyte can be moisture in itself.Because space is less between the effective surface area of porous material and electrode, therefore, for the capacitor obtained, bulky capacitor value can be had.But often the problem relevant to this type of electric capacity is: when aqueous electrolyte exposes in high temperature environments, easily occur thermal expansion.This can cause electrolyte to be revealed from capacitor, and conversely, this result in again capacitance and reduces and equivalent series resistance increase.Therefore, need now to improve double layer capacitor, even if when making it expose at high temperature, also show good electrical characteristic.
Summary of the invention
According to one embodiment of the invention, propose the double layer capacitor that one comprises an electrochemical cell (electrochemical cell), this electrochemical cell comprises the first and second electrodes, and wherein each electrode comprises a kind of porous matrix of electro-chemical activity particulate separately.This electrochemical cell also comprises a kind of aqueous electrolyte, arranges in contact with above-mentioned electro-chemical activity particulate.Electrolyte comprises a kind of anionic polymer and a kind of polyacid.According to another embodiment of the present invention, propose a kind of method of the electrochemical cell for the formation of double layer capacitor, the method comprises: arrange a paste in contact with electrode, wherein this paste comprises electro-chemical activity particulate and aqueous electrolyte, and this electrolyte comprises a kind of polyacid and a kind of anionic polymer.
Other characteristic sum aspects of the present invention, are provided by following more detailed description.
Accompanying drawing explanation
For those skilled in the art, set forth in more detail in the remainder of the description and comprised the of the present invention complete and effective open of best execution mode, and have references to accompanying drawing, wherein:
Fig. 1 is the cutaway view of an embodiment of capacitor according to formation of the present invention; And
Fig. 2 is the exploded view of an embodiment of electrochemical cell in capacitor used in the present invention;
Same or analogous Reference numeral in this specification and accompanying drawing represents same or analogous technical characteristic of the present invention or element.
Embodiment
It will be appreciated by those skilled in the art that discussed herein is only the description of exemplary embodiment, but not to of the present invention embody to some extent in the structure that this is exemplary wider in restriction.
Generally speaking, the present invention relates to a kind of double layer capacitor comprising at least one electrochemical cell.Electrochemical cell comprises multiple electrode (such as, 2 electrodes), and wherein each electrode comprises the porous matrix of an electro-chemical activity particulate (such as, carbon).A kind of aqueous electrolyte and porous matrix are set up in contact.According to the present invention, electrolyte is configured with the adhesive that an anionic polymer is used as electro-chemical activity particulate, can reduce electrolytical loss, the loss especially when high temperature with this.Because condensate is anion-containing in itself, so it is normally hydrophilic, therefore also just can still keep its adhesiveness when meeting water.Polymeric anion essence also makes it keep stable when running into corrosivity polyacid, and this polyacid is used in electrolyte to improve charge density.Therefore, as result of the present invention, the capacitor formed can demonstrate good electric property (such as, high capacity and low ESR), even if under high temperature (such as, 70 DEG C and higher temperature), still possess the electric property that this is good.
Anionic polymer for aqueous electrolyte typically comprises one or more anionic functional group, and this anionic functional group can suspend (pendant from) in midair outside polymeric backbone (polymer backbone) and/or be contained among polymeric backbone (polymer backbone).Suitable anionic group can comprise, such as, and carboxylate (carboxylate), sulfonate (sulfonate), sulfate (sulphate), and/or other electronegative ionizing groups arbitrarily.Polymeric backbone can be formed by multiple different monomers, such as, and aromatic monomer, aliphatic monomer and combination thereof.The monomer being especially suitable for being formed anionic polymer is vinyl aromatic monomer (vinyl aromatic monomers), such as, styrene, 2-vinyl naphthalene (2-vinyl naphthalene), AMS (alpha-methyl styrene), 3-methyl styrene (3-methylstyrene), 4-methyl styrene (4-methylstyrene), 2, 4-dimethyl styrene (2, 4-dimethylstyrene), 2, 5-dimethyl styrene (2, 5-dimethylstyrene), 3, 5-dimethyl styrene (3, 5-dimethylstyrene), 2, 4, 6-trimethyl styrene (2, 4, 6-trimethylstyrene), 4-tert-butyl styrene (4-tert-butylstyrene), 4-methoxy styrene (4-methoxystyrene), 4-ethoxystyrene (4-ethoxystyrene), 2-chlorostyrene (2-chlorostyrene), 3-chlorostyrene (3-chlorostyrene), 4-chlorostyrene (4-chlorostyrene), 2, 6-dichlorostyrene (2, 6-dichlorostyrene), 4-bromstyrol (4-bromostyrene), 4-acetoxy-styrene (4-acetoxystyrene), 4-Vinyl phenol (4-hydroxystyrene), 4-aminostyryl (4-amino styrene), to dimethylethyloxy siloxy styrene (p-dimethylethoxy siloxy styrene), 2-vinylpyridine (2-vinyl pyridine), 4-vinylpridine (4-vinyl pyridine), vinyl benzoate (vinyl benzoate), the vinyl benzoic acid 4-tert-butyl ester (vinyl 4-tert-butyl benzoate), vinylcarbazole (vinyl carbazole), vinyl ferrocene (vinyl ferrocene) etc.The object lesson of this kind of anionic polymer comprises: sulfonated polymer body, such as, poly-(styrene sulfonic acid) (poly (styrenesulfonic acid), poly-(2-acrylic-amino-2-methyl isophthalic acid-propane sulfonic acid) (poly (2-acrylamido-2-methyl-1-propane sulfonic acid)), sulfonation gathers (ether ether ketone) (sulfonated poly (etheretherketone)), sulfonated lignin (sulfonated lignin), poly-(vinyl sulfonic acid) (poly (ethylenesulfonic) acid), poly-(methacrylic acid ethyoxyl sulfonic acid) (poly (methacryloxyethylsulfonic acid)) etc., carboxylated polymer (carboxylated polymers), such as poly-(acrylic acid), poly-(methacrylic acid) (poly (methacrylic acid)), etc.Sulfated polymeric body, such as carrageenan (carrageenan) etc.; The salt of any aforementioned polymer, and combination.This kind of polymeric salt can comprise, such as, and metal cation, such as sodium, potassium, calcium, lithium, caesium, zinc, copper, iron, aluminium, zirconium, lanthanum, yttrium, magnesium, strontium, cerium etc.The object lesson of this kind of salt comprises, and such as, or gathers (styrene sulfonic acid) lithium salts or sodium salt.
As implied above, aqueous electrolyte also comprises a polyacid, and it can stand two or more times proton dissociation (such as, 2 times, 3 is inferior).The example of some polyacids be applicable to can be applicable to herein, such as, hydrogen sulfide (binary), sulfuric acid (binary), sulfurous acid (binary), phosphoric acid (ternary), ethanedioic acid (binary), carbonic acid (binary), malonic acid (binary) etc.Sulfuric acid (H 2sO 4) passable, such as, lose a proton to form hydrogen sulfate anion (HSO 4 -), lose second proton and form sulfate anion (SO 4 2-).Certainly, electrolyte can also comprise monoacid compound, such as, and nitric acid, nitrous acid, hydrochloric acid, perchloric acid, hydroiodic acid, hydrofluoric acid etc.
The relative concentration of electrolyte components is selected to obtain the balance of the electrical characteristic of capacitor usually.Such as, although high anionic polymerization bulk concentration can improve electrolyte be exposed to stability in high temperature, too high concentration but can have negative effect to the capacitance of electrolytical conductivity and the capacitor obtained thus.Consider this point, the invention discloses polyacid relative to the weight ratio of anionic polymer is about 2: 1 to about 40: 1, in certain embodiments, and about 5: 1 to about 30: 1, and in certain embodiments, use the percentage by weight of about 10: 1 to about 20: 1 to obtain the electric property expected.Such as, anionic polymer can account for electrolytical about 0.05wt.% to about 15wt.%, in certain embodiments, and about 0.1wt.% to about 10wt.%, in certain embodiments, about 0.5wt.% to about 5wt.%.Same, polyacid can account for electrolytical about 10wt.% to about 70wt.%, in certain embodiments, and about 20wt.% to about 60wt.%, and in certain embodiments, about 25wt.% to about 50wt.%.
Aqueous electrolyte usually can in a variety of forms in any one form exist, such as, solution, dispersion, gelinite etc.But, no matter what kind of its form existed is, aqueous electrolyte typically accounts for electrolyte (such as, anionic polymer, polyacid containing weight, and water) component about 30wt.% to about 90wt.% water (such as, deionized water), in certain embodiments, be about 40wt.% to about 80wt.%, in further embodiments, 50wt.% to about 70wt.% is about.The aqueous electrolyte obtained can have about 10milliSiemens/ centimetre (" mS/cm ") or larger electric conductivity, in further embodiments, about 30mS/cm or larger, in further embodiments, about 40mS/cm to about 100mS/cm, above-mentioned data for record at 25 DEG C.The numerical value of electric conductivity records 25 DEG C time by using any existing electric conductivity meter (such as, Oakton Con 11 series).
The electro-chemical activity particulate used in the electrode of capacitor is configured to the effective surface area increasing electrode.The effective surface area of this increase makes the formation of capacitor have larger cell capacitance amount to a given volume and/or make the formation of capacitor have less volume to a given capacitance.Typically, electro-chemical activity particulate has one and is specifically about 200m 2the surface area of/g, in certain embodiments, is about 500m 2/ g, in further embodiments, is at least about 1500m 2/ g.For obtaining the surface area expected, electro-chemical activity particulate has small size usually.Such as, the medium volume of electro-chemical activity particulate can be less than about 100 microns, in certain embodiments, and about 0.01 to about 50 micron, in further embodiments, about 0.1 to about 20 micron.Same, electro-chemical activity particulate can be porous form.Such as, electro-chemical activity particulate can have hole or the passage that multiple average diameter is greater than about 5 dusts (angstrom), and in certain embodiments, above-mentioned diameter is greater than about 20 dusts, in certain embodiments, is greater than about 50 dusts.
In multiple electro-chemical activity particulate, any one can be used in the present invention.Such as, the carbon particulate of the level of conductivity with expectation can be used, such as, activated carbon, carbon black, graphite, carbon nano-tube (carbon nanotube) etc., with and composition thereof.The form of some active carbons be suitable for and form technology at the United States Patent(USP) Nos. 5,726,118 of the people such as Ivey; The United States Patent (USP) 5,858,911 of the people such as Wellen, and involved by having in the open text No.2003/0158342 of the U.S. Patent application of the people such as Shinozaki, the mode that foregoing is quoted in full is introduced in this as a reference.Various metals also can be used as electro-chemical activity particulate, such as, by ruthenium, and iridium, nickel, rhodium, rhenium, cobalt, tungsten, manganese, tantalum, niobium, molybdenum, plumbous, titanium, platinum, palladium and osmium, and the particulate that the combination of above-mentioned metal is formed.Also the nonisulated oxide fine particle by reversible faraday's reaction sequence (reversible faradaic reaction sequence) generation current can be used.The oxide be suitable for can comprise a kind of metal, and this metal is selected from ruthenium, iridium, nickel, rhodium, rhenium, cobalt, tungsten, manganese, tantalum, niobium, molybdenum, aluminium, plumbous, titanium, platinum, the combination of a kind of or above-mentioned metal in palladium and osmium, the metal oxide be especially suitable in the present invention comprises ruthenic oxide (RuO 2).
Electro-chemical activity particulate is general to be set up in contact with an electrode, and it can by different electric conducting materials, as tantalum, and niobium, aluminium, nickel, hafnium, titanium, copper, silver, aluminium, steel (as stainless steel), and any one in its alloy (as conductive oxide) etc. is formed.Titanium, and its alloy, be particluarly suitable for use of the present invention.As is known to the person skilled in the art, the geometrical construction of this electrode (electrode) generally can change to some extent, such as, with a container, tank (can), paper tinsel (foil), thin slice (sheet), sieve (screen), the forms such as framework (frame) exist.
The capacitor obtained can have any desired structure as known in the art.With reference to figure 1, such as, an embodiment of a double layer capacitor 10 is schematically shown, and it comprises the aqueous electrolyte 20 contacted with the second electrode 42 with the first electrode 32.First electrode 32 is coated with the porous matrix of one deck electro-chemical activity particulate 34.Similarly, the second electrode 42 is coated with the porous matrix of one deck electro-chemical activity particulate 44.Typically, about 10 microns to 1000 microns of the interval be set up between electrode 32 and 42.In this particular embodiment, a spacer 50 is also provided with between electrode to suppress the short circuit of the electric charge assembled on two electrodes.Spacer 50 has permeability to flow through to allow the ionic current of electrolyte 20.The example of suitable material for this purpose comprises, such as, porous polymeric body material (such as, polypropylene, polyethylene etc.), porous inorganic material (as fiberglass packing (fiberglass mats), porous glass paper (porous glass paper) etc.), ion exchange resin material etc.Special example comprises ion perfluorinated sulfonic acid polymeric films (as the Nafion that Du Pont (DuPont) produces tMfilm), sulfonation fluorine carbon polymeric films, polybenzimidazoles (PBI) film, and polyether-ether-ketone (PEEK) film.
As known in the art, the generation type of double layer capacitor, also can have multiple different mode.In one embodiment, such as, first aqueous electrolyte and electro-chemical activity particulate are mixed to form paste.Solids in paste, typically, accounts for the about 5wt.% of paste to about 55wt.%, in certain embodiments, and about 10wt.% to about 50wt.%, in certain embodiments, about 15wt.% to about 40wt.%.Such as, electro-chemical activity particulate (such as, carbon black, graphite, etc.) typically account for the about 5wt.% of this paste to about 50wt.%, in certain embodiments, about 10wt.% to about 40wt.%, in certain embodiments, about 15wt.% to about 30wt.%.Aqueous electrolyte also can account for the about 50wt.% of this paste to about 95wt.%.In certain embodiments, about 60wt.% to about 90wt.%, in certain embodiments, about 70wt.% to about 85wt.%.Such as, anionic polymer can account for the about 0.01wt.% of this paste to about 10wt.%, in certain embodiments, and about 0.05wt.% to about 4wt.%, and in certain embodiments, about 0.2wt.% to about 2wt.%; Polyacid can account for the about 10wt.% of this paste to about 40wt.%, in certain embodiments, and about 15wt.% to about 35wt.%, and in certain embodiments, about 20wt.% to about 30wt.%; And water can account for the about 30wt.% of this paste to about 70wt.%, in certain embodiments, about 35wt.% to about 65wt.%, and in certain embodiments, about 40wt.% to about 60wt.%.
Once be formed, then by such as printing (printing) (such as, photocopy (rotogravure)), spraying (spraying), groove film coating (slot-die coating), drip be coated with (drop-coating), any known technologies useful such as dip-coating (dip-coating) by this paste for electrode.With reference to figure 2, such as, the embodiment of the method for an integrated electrochemical battery 100 is shown.In this embodiment, paste 126 is begun to take shape by the mixture of aqueous electrolyte and electro-chemical activity particulate.Then, paste 126 and an electrode 128 are arranged in the opening of an insulation system 120 (being pointed out by the arrow in band direction), and insulation system 120 is then connected to another electrode 124.As the United States Patent (USP) 6 of the people such as United States Patent(USP) Nos. 6,790,556 and Meitav of the people such as Meitav, 576, described in 365 to, structure 120 can be non-conductive with perforation in essence, and the mode that foregoing is quoted in full is introduced in this as a reference.
Above-described embodiment normally relates to and uses single electrochemical cell in the capacitor.But, certainly should be appreciated that capacitor of the present invention also can comprise the electrochemical cell of more than 2 or 2.In one such embodiment, such as, capacitor can comprise the electrochemical cell of a pile more than 2 or 2, and these electrochemical cells can be identical or different.
Regardless of the ad hoc structure of double layer capacitor of the present invention, this double layer capacitor all can have excellent electrical characteristic, even if be also at high temperature like this.Such as, capacitor of the present invention can have about 100 ohm (ohm) or less equivalent series resistance (ESR), in certain embodiments, about 50 ohm or less, in certain embodiments, about 0.01 to about 500 milliohm (milliohms), in certain embodiments, about 0.1 to about 100 milliohm, and in further embodiments, about 0.1 to about 50 milliohm, above-mentioned data all record under the operating frequency of 120Hz.Similarly, capacitance can be about 1 millifarad/centimetre 2(" mF/cm 2") or larger, in certain embodiments, about 2mF/cm 2or larger, in certain embodiments, about 5 to about 50mF/cm 2, and in further embodiments, about 8 to about 20mF/cm 2, the numerical value of these equivalent series resistances and capacitance even at high temperature also can remain unchanged.Such as, these numerical value can remain unchanged under about 60 DEG C of temperature ranges to about 80 DEG C (such as, 70 DEG C).
This capacitor can be widely used in various application occasions, such as Medical Devices (such as, implanted defibrillator, cardiac pacemaker, cardioverter, nerve stimulator, medication administration device etc.); Automation application; Military Application (such as, radar system); The equipment of consumer electronics (such as, broadcast receiver, television set etc.) and the like.In one embodiment, such as, capacitor can be used in implantable medical device, these Medical Devices be configured to patient provide treatment high voltage (as at about 500V to about between 850V, or, ideally, at about 600V to about between 800V) and treatment.This equipment can comprise and sealed and have container or the housing of biologically inert.One or more wire is electrically connected by vein between equipment and patient's heart.There is provided heart electrode to detect cardiomotility and/or to provide voltage to heart.At least part of wire (e.g., the tail end of wire) can with in the ventricle of heart and atrium one or more near to or in contact with.This equipment also comprises a Capacitor banks, generally includes the capacitor of two or more series connection, and they are connected with the battery of device interior or outside, and described battery provides energy to described Capacitor banks.
The present invention can better be illustrated by following examples.
testing procedure
Equivalent series resistance (ESR) and capacitance:
The Agilent LCR of Kelvin or equivalent 4 points (source and induction end) probe structure table (model 4263B) is used to measure equivalent series resistance.Measure setup is: pattern: Rs, the time: long, direct current biasing: 0V, frequency: 1000Hz and LVL:1000mV.Before measurement, that once opens a way compensates with short circuit, and the internal algorithm that this compensation uses the LCR that Agilent model is 4263B to show eliminates the impact of wire length and probe contacts resistance.Use with the specified equivalent series resistance of capacitor close, allow the resistance of the error of 1% to carry out resistance measurement.Four-point probe being all connected with capacitor, by triggering LCR table, can equivalent series resistance being recorded.
Use Keithley source table (model: 2400 or 2601 or 2602) measure capacitance.Need during measurement fully to charge to its rated voltage to capacitor, and charging is until charging current is lower than 1mA.These parts stablize 5 minutes under open-circuit condition.Discharge from 4mA electric current, and sustain discharge electric current 4mA ground discharges.Twice voltage readings using interval to be at least 1 second calculates.By using formulae discovery below to determine capacitance: capacitance=| Δ t|*I/| Δ V|.
embodiment 1
Demonstrate a kind of method forming the conductive paste used in capacitor of the present invention.First, by the carbon black powders of 18 grams of high surface areas and 6 grams of powdered graphite (production of Sigma Aldrich company) mixing.In addition, by 4M sulfuric acid (the 4M H of 64.8 grams 2sO 4) slowly add 7.2 grams of moisture gathering in (styrene sulfonic acid) (concentration is 18wt.%) solution.Above-mentioned acidic mixture is added carbon mix and be that the cylinder of 30rpm makes it fully mix by preparation being placed in a rotating speed.Use the paste of the abundant description in the United States Patent(USP) Nos. 6,790,556 and 6,576,365 of Meitav etc., one group of 6 monocell can be made.Thereafter, to 10 groups of above-mentioned batteries, under 85 DEG C and rated voltage 4.5V condition, test its equivalent series resistance and capacitance, result is as shown in following table 1 and 2:
Table 1
Table 2
embodiment 2
Demonstrate a kind of method forming the conductive paste used in capacitor of the present invention.First, by the carbon black powders of 9.7 grams of high surface areas and 3.3 grams of powdered graphite (production of Sigma Aldrich company) mixing.In addition, by 4M sulfuric acid (the 4M H of 82 grams 2sO 4) slowly add 9.1 grams of moisture gathering in (styrene sulfonic acid) (concentration is 18wt.%) solution.Above-mentioned acidic mixture is added carbon mix and by preparation is placed in a rotating speed be 30rpm cylinder maintenance 24 hours, make it fully mix.After making, form 16 monocells by conductive paste, its area is 40.5mmx22.5mm.One Battery pack is placed in about 1340 hours (8 weeks) in 70 DEG C, and another group is placed in about 1340 hours (8 weeks) in 25 DEG C.Above-mentioned battery tests weekly once its equivalent series resistance and capacitance.The test result of 8 weeks as shown in Table 3, 4.
Table 3: be stored in the monocell in 70 DEG C
Table 4: be stored in the monocell in 25 DEG C
embodiment 3
Demonstrate a kind of method forming the conductive paste used in capacitor of the present invention.First, the carbon black powders of 30.1 grams of high surface areas and 10 grams of powdered graphites (production of Sigma Aldrich company) are mixed and rocked for 10 seconds.In addition, the 5M sulfuric acid of 169.9 grams is slowly added 19.1 grams of moisture gathering in (styrene sulfonic acid) (concentration is 18wt.%) solution.Above-mentioned acidic mixture is added in carbon mix, and stirs to guarantee that wherein carbon mix is fully moistening with glass bar.
embodiment 4
Demonstrate a kind of method forming the conductive paste used in capacitor of the present invention.First, by the carbon black powders of 17 grams of high surface areas and 3 grams of powdered graphite (production of Sigma Aldrich company) mixing, and rocked for 10 seconds.In addition, by poly-(styrene sulfonic acid) sodium salt (~ M of 2 grams w70000) (production of Sigma Aldrich company) mix with 7 grams of moisture poly-(styrene sulfonic acid) (concentration is 18wt.%) solution.Then, 80 grams of 5M sulfuric acid are added in said mixture.Above-mentioned acidic mixture is added in carbon mix, and stirs to guarantee that wherein carbon mix is fully moistening with glass bar.The acidic mixture obtained is placed in a rotating speed be 30rpm cylinder keep 24 hours.After making, form 16 monocells by conductive paste, its area is 40.5mmx22.5mm.One Battery pack is placed in about 1340 hours (8 weeks) in 70 DEG C, and another group is placed in about 1340 hours (8 weeks) in 25 DEG C.Above-mentioned battery tests weekly once its equivalent series resistance and capacitance.The test result of 8 weeks as shown in Table 5,6.
Table 5: be stored in the monocell in 70 DEG C
Table 6: be stored in the monocell in 25 DEG C
Modification and the distortion of the invention described above can be determined according to the common technology of this area, and do not deviate from the spirit and scope of the present invention.In addition, it will be appreciated that, each side of different embodiment can be replaced in whole or in part mutually.And those skilled in the art should know, above-mentioned record, only for example, can not limit the scope of the present invention and claim.

Claims (25)

1. a double layer capacitor, comprises an electrochemical cell, this battery:
First and second electrodes, comprise the porous matrix of an electro-chemical activity particulate separately, and wherein said electro-chemical activity particulate comprises carbon particulate, by ruthenium, iridium, nickel, rhodium, rhenium, cobalt, tungsten, manganese, tantalum, niobium, molybdenum, plumbous, titanium, platinum, the particulate that the combination of palladium and osmium or above-mentioned metal is formed, by the reversible nonisulated oxide fine particle of faraday's reaction sequence generation current or the combination of above-mentioned particulate; And
One aqueous electrolyte, this aqueous electrolyte and described electro-chemical activity particulate are set up in contact, wherein, described electrolyte comprises an anionic polymer and a polyacid, wherein said anionic polymer comprises sulfate, carboxylate or sulfonic acid functional group, and described polyacid can stand two or more times proton dissociation.
2. double layer capacitor as claimed in claim 1, wherein said anionic polymer is formed by vinyl aromatic monomer.
3. double layer capacitor as claimed in claim 2, wherein, described vinyl aromatic monomer is styrene.
4. the double layer capacitor as described in one of aforementioned claim, wherein, described anionic polymer comprises poly-(styrene sulfonic acid), the salt of poly-(styrene sulfonic acid), or its mixture.
5. double layer capacitor as claimed in claim 1, wherein, described polyacid comprises sulfuric acid.
6. double layer capacitor as claimed in claim 1, wherein, in described electrolyte, described polyacid is 2: 1 to 40: 1 relative to the weight ratio of described anionic polymer.
7. double layer capacitor as claimed in claim 1, wherein, in described electrolyte, described polyacid is 10: 1 to 20: 1 relative to the weight ratio of described anionic polymer.
8. double layer capacitor as claimed in claim 1, wherein, described anionic polymer accounts for the 0.05wt.% to 15wt.% of described aqueous electrolyte, and described polyacid accounts for the 10wt.% to 70wt.% of described aqueous electrolyte.
9. double layer capacitor as claimed in claim 1, wherein, described anionic polymer accounts for the 0.5wt.% to 5wt.% of described aqueous electrolyte, and described polyacid accounts for the 25wt.% to 50wt.% of described aqueous electrolyte.
10. double layer capacitor as claimed in claim 1, wherein, water accounts for described electrolytical 30wt.% to 90wt.%.
11. double layer capacitors as claimed in claim 1, wherein, water accounts for described electrolytical 50wt.% to 70wt.%.
12. double layer capacitors as claimed in claim 1, wherein, described electrode comprises titanium.
13. double layer capacitors as claimed in claim 1, wherein, described battery also comprises one infiltrative spacer, and this spacer is arranged between described electrode.
14. double layer capacitors as claimed in claim 1, wherein, described capacitor comprises multiple electrochemical cell.
15. double layer capacitors as claimed in claim 1, wherein, measure at the temperature of the operating frequency of 120Hz and 70 DEG C, described capacitor has 100 ohm or less equivalent series resistance.
16. double layer capacitors as claimed in claim 1, wherein, measure at the temperature of the operating frequency of 120Hz and 70 DEG C, described capacitor has the equivalent series resistance of 0.1 to 50 milliohm.
17. double layer capacitors as claimed in claim 1, wherein, described capacitor have at 70 DEG C of temperature 1 millifarad/centimetre 2or larger capacitance.
18. double layer capacitors as claimed in claim 1, wherein, described capacitor have at 70 DEG C of temperature 5 to 50 millifarads/centimetre 2capacitance.
19. 1 kinds of methods for the formation of the electrochemical cell of double layer capacitor, the method comprises: arrange a paste in contact with an electrode, wherein, described paste comprises a kind of electro-chemical activity particulate and a kind of aqueous electrolyte, wherein said electro-chemical activity particulate comprises carbon particulate, by ruthenium, iridium, nickel, rhodium, rhenium, cobalt, tungsten, manganese, tantalum, niobium, molybdenum, plumbous, titanium, platinum, the particulate that the combination of palladium and osmium or above-mentioned metal is formed, by the nonisulated oxide fine particle of reversible faraday's reaction sequence generation current, or the combination of above-mentioned particulate, described electrolyte comprises a polyacid and an anionic polymer, wherein said polyacid can stand two or more times proton dissociation, described anionic polymer comprises sulfate, carboxylate or sulfonic acid functional group.
20. methods as claimed in claim 19, wherein, described anionic polymer is formed by a styrene monomer.
21. methods as claimed in claim 19, wherein, described anionic polymer comprises poly-(styrene sulfonic acid), the salt of poly-(styrene sulfonic acid), or its mixture.
22. methods as claimed in claim 19, wherein, described polyacid comprises sulfuric acid.
23. methods as claimed in claim 19, wherein, the described polyacid in described paste is 2: 1 to 40: 1 relative to the weight ratio of described anionic polymer.
24. methods as claimed in claim 19, wherein, the described polyacid in described paste is 10: 1 to 20: 1 relative to the weight ratio of described anionic polymer.
25. methods as claimed in claim 19, wherein, described electrode comprises titanium.
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